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Extreme ultraviolet (EUV) photon beam characterization techniques, Hartmann wavefront sensing and single shot ablation imprinting, were compared along the caustic of a tightly focused free-electron laser (FEL) beam at beamline FL24 of FLASH2, the Free-electron LASer in Hamburg at DESY. The transverse coherence of the EUV FEL was determined by a Young's double pinhole experiment and used in a back-propagation algorithm which includes partial coherence to calculate the beam intensity profiles along the caustic from the wavefront measurements. A very good agreement of the profile structure and size is observed for different wavelengths between the back-propagated profiles, an indirect technique, and ablation imprints. As a result, the Hartmann wavefront sensor including its software MrBeam is a very useful, single shot pulse resolved and fast tool for non-invasive determination of focal spot size and shape and also for beam profiles along the caustic.

A change of orbital state alters the coupling between ions and their surroundings drastically. Orbital excitations are hence key to understand and control interaction of ions. Rare-earth elements with strong magneto-crystalline anisotropy (MCA) are important ingredients for magnetic devices. Thus, control of their localized 4 f magnetic moments and anisotropy is one major challenge in ultrafast spin physics. With time-resolved x-ray absorption and resonant inelastic scattering experiments, we show for Tb metal that 4 f -electronic excitations out of the ground-state multiplet occur after optical pumping. These excitations are driven by inelastic 5 d -4 f -electron scattering, altering the 4 f -orbital state and consequently the MCA with important implications for magnetization dynamics in 4 f -metals and more general for the excitation of localized electronic states in correlated materials.

Identifying the microscopic nature of non-equilibrium energy transfer mechanisms among electronic, spin, and lattice degrees of freedom is central to understanding ultrafast phenomena such as manipulating magnetism on the femtosecond timescale. Here, we use time- and angle-resolved photoemission spectroscopy to go beyond the often-used ensemble-averaged view of non-equilibrium dynamics in terms of quasiparticle temperature evolutions. We show for ferromagnetic Ni that the non-equilibrium electron and spin dynamics display pronounced variations with electron momentum, whereas the magnetic exchange interaction remains isotropic. This highlights the influence of lattice-mediated scattering processes and opens a pathway toward unraveling the still elusive microscopic mechanism of spin-lattice angular momentum transfer.

Methods of ablation imprints in solid targets are widely used to characterize focused X-ray laser beams due to a remarkable dynamic range and resolving power. A detailed description of intense beam profiles is especially important in high-energy-density physics aiming at nonlinear phenomena. Complex interaction experiments require an enormous number of imprints to be created under all desired conditions making the analysis demanding and requiring a huge amount of human work. Here, for the first time, we present ablation imprinting methods assisted by deep learning approaches. Employing a multi-layer convolutional neural network (U-Net) trained on thousands of manually annotated ablation imprints in poly(methyl methacrylate), we characterize a focused beam of beamline FL24/FLASH2 at the Free-electron laser in Hamburg. The performance of the neural network is subject to a thorough benchmark test and comparison with experienced human analysts. Methods presented in this Paper pave the way towards a virtual analyst automatically processing experimental data from start to end.

Extending nonlinear spectroscopic techniques into the x-ray domain promises unique insight into photoexcited charge dynamics, which are of fundamental and applied interest. We report on the observation of a third-order nonlinear process in lithium fluoride (LiF) at a free-electron laser. Exploring the yield of four-wave mixing (FWM) in resonance with transitions to strongly localized core exciton states versus delocalized Bloch states, we find resonant FWM to be a sensitive probe for the degree of charge localization: Substantial sum- and difference-frequency generation is observed exclusively when in a one- or three-photon resonance with a LiF core exciton, with a dipole forbidden transition affecting details of the nonlinear response. Our reflective geometry-based approach to detect FWM signals enables the study of a wide variety of condensed matter sample systems, provides atomic selectivity via resonant transitions, and can be easily scaled to shorter wavelengths at free-electron x-ray lasers.

X-ray absorption near-edge structure (XANES) spectroscopy provides element specificity and is a powerful experimental method to probe local unoccupied electronic structures. In the soft x-ray regime, it is especially well suited for the study of 3 d -metals and light elements such as nitrogen. Recent developments in vacuum-compatible liquid flat jets have facilitated soft x-ray transmission spectroscopy on molecules in solution, providing information on valence charge distributions of heteroatoms and metal centers. Here, we demonstrate XANES spectroscopy of molecules in solution at the nitrogen K -edge, performed at FLASH, the Free-Electron Laser (FEL) in Hamburg. A split-beam referencing scheme optimally characterizes the strong shot-to-shot fluctuations intrinsic to the process of self-amplified spontaneous emission on which most FELs are based. Due to this normalization, a sensitivity of 1% relative transmission change is achieved, limited by fundamental photon shot noise. The effective FEL bandwidth is increased by streaking the electron energy over the FEL pulse train to measure a wider spectral window without changing FEL parameters. We propose modifications to the experimental setup with the potential of improving the instrument sensitivity by two orders of magnitude, thereby exploiting the high peak fluence of FELs to enable unprecedented sensitivity for femtosecond XANES spectroscopy on liquids in the soft x-ray spectral region., (© 2021 Author(s).)

An extreme-ultraviolet (XUV) double-stage Raman spectrometer is permanently installed as an experimental end-station at the PG1 beamline of the soft X-ray/XUV free-electron laser in Hamburg, FLASH. The monochromator stages are designed according to the Czerny-Turner optical scheme, adapted for the XUV photon energy range, with optical elements installed at grazing-incidence angles. Such an optical scheme along with the usage of off-axis parabolic mirrors for light collimation and focusing allows for aberration-free spectral imaging on the optical axis. Combining the two monochromators in additive dispersion mode allows for reaching high resolution and superior stray light rejection, but puts high demands on the quality of the optical alignment. In order to align the instrument with the highest precision and to quantitatively characterize the instrument performance and thus the quality of the alignment, optical laser interferometry, Hartmann-Shack wavefront-sensing measurements as well as off-line soft X-ray measurements and extensive optical simulations were conducted. In this paper the concept of the alignment scheme and the procedure of the internal optical alignment are presented. Furthermore, results on the imaging quality and resolution of the first monochromator stage are shown.

The non-monochromatic beamline BL1 at the FLASH free-electron laser facility at DESY was upgraded with new transport and focusing optics, and a new permanent end-station, CAMP, was installed. This multi-purpose instrument is optimized for electron- and ion-spectroscopy, imaging and pump-probe experiments at free-electron lasers. It can be equipped with various electron- and ion-spectrometers, along with large-area single-photon-counting pnCCD X-ray detectors, thus enabling a wide range of experiments from atomic, molecular, and cluster physics to material and energy science, chemistry and biology. Here, an overview of the layout, the beam transport and focusing capabilities, and the experimental possibilities of this new end-station are presented, as well as results from its commissioning., (open access.)

The extreme-ultraviolet double-stage imaging Raman spectrometer is a permanent experimental endstation at the plane-grating monochromator beamline branch PG1 at FLASH at DESY in Hamburg, Germany. This unique instrument covers the photon energy range from 20 to 200 eV with high energy resolution of about 2 to 20 meV (design values) featuring an efficient elastic line suppression as well as effective stray light rejection. Such a design enables studies of low-energy excitations like, for example, phonons in solids close to the vicinity of the elastic line. The Raman spectrometer effectively operates with four reflective off-axial parabolic mirrors and two plane-grating units. The optics quality and their precise alignment are crucial to guarantee best performance of the instrument. Here, results on a comprehensive investigation of the quality of the spectrometer diffraction gratings are presented. The gratings have been characterized by ex situ metrology at the BESSY-II Optics Laboratory, employing slope measuring deflectometry and interferometry as well as atomic force microscopy studies. The efficiency of these key optical elements has been measured at the at-wavelength metrology laboratory using the reflectometer at the BESSY-II Optics beamline. Also, the metrology results are discussed with respect to the expected resolving power of the instrument by including them in ray-tracing studies of the instrument.

The stochastic nature of the self-amplified spontaneous emission (SASE) process of free-electron lasers (FELs) effects pulse-to-pulse fluctuations of the radiation properties, such as the photon energy, which are determinative for processes of photon-matter interactions. Hence, SASE FEL sources pose a great challenge for scientific investigations, since experimenters need to obtain precise real-time feedback of these properties for each individual photon bunch for interpretation of the experimental data. Furthermore, any device developed to deliver the according information should not significantly interfere with or degrade the FEL beam. Regarding the spectral properties, a device for online monitoring of FEL wavelengths has been developed for FLASH2, which is based on photoionization of gaseous targets and the measurements of the corresponding electron and ion time-of-flight spectra. This paper presents experimental studies and cross-calibration measurements demonstrating the viability of this online photoionization spectrometer.

The Kirkpatrick-Baez (KB) refocusing mirror system installed at the PG1 branch of the plane-grating monochromator beamline at the soft X-ray/XUV free-electron laser in Hamburg (FLASH) is designed to provide tight aberration-free focusing down to 4 µm × 6 µm full width at half-maximum (FWHM) on the sample. Such a focal spot size is mandatory to achieve ultimate resolution and to guarantee best performance of the vacuum-ultraviolet (VUV) off-axis parabolic double-monochromator Raman spectrometer permanently installed at the PG1 beamline as an experimental end-station. The vertical beam size on the sample of the Raman spectrometer, which operates without entrance slit, defines and limits the energy resolution of the instrument which has an unprecedented design value of 2 meV for photon energies below 70 eV and about 15 meV for higher energies up to 200 eV. In order to reach the designed focal spot size of 4 µm FWHM (vertically) and to hold the highest spectrometer resolution, special fully motorized in-vacuum manipulators for the KB mirror holders have been developed and the optics have been aligned employing wavefront-sensing techniques as well as ablative imprints analysis. Aberrations like astigmatism were minimized. In this article the design and layout of the KB mirror manipulators, the alignment procedure as well as microfocus optimization results are presented.

The design and the commissioning results of a portable and compact spectrometer for the high harmonics content characterization of the extreme-ultraviolet radiation of FLASH (free-electron laser in DESY, Hamburg, Germany) are presented. The instrument is a grazing-incidence flat-field spectrometer equipped with two variable-line-spaced gratings; it covers the 2-40 nm wavelength region with a spectral resolution in the 0.1-0.2% range. Both spectral and intensity fluctuations of the fundamental emission and the harmonics are monitored.